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MXPA97003994A - Stabilization of organic peroxide with fosfomolibd acid - Google Patents

Stabilization of organic peroxide with fosfomolibd acid

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Publication number
MXPA97003994A
MXPA97003994A MXPA/A/1997/003994A MX9703994A MXPA97003994A MX PA97003994 A MXPA97003994 A MX PA97003994A MX 9703994 A MX9703994 A MX 9703994A MX PA97003994 A MXPA97003994 A MX PA97003994A
Authority
MX
Mexico
Prior art keywords
peroxydicarbonate
organic peroxide
phosphomolybdic acid
butyl
weight
Prior art date
Application number
MXPA/A/1997/003994A
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Spanish (es)
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MX9703994A (en
Inventor
Frenkel Peter
Abma Charles
Original Assignee
Witco Corporation
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Priority claimed from US08/656,095 external-priority patent/US5719304A/en
Application filed by Witco Corporation filed Critical Witco Corporation
Publication of MX9703994A publication Critical patent/MX9703994A/en
Publication of MXPA97003994A publication Critical patent/MXPA97003994A/en

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Abstract

The present invention relates to organic peroxide compositions containing phosphomolybdic acid to retard the decomposition rate of the peroxy compound

Description

STABILIZATION OF ORGANIC PEROXIDE WITH PHOSPHOMOLYBIC ACID BACKGROUND OF THE INVENTION The present invention relates to organic peroxide compositions and more specifically to peroxydicarbonate compositions, wherein phosphomolybdic acid has been added to retard the rate of decomposition of the peroxide compound. Organic peroxides such as peroxydicarbonates are useful as free radical initiators in the polymerization or copolymerization of ethylenically unsaturated monomers. For example, organic peroxides are used as initiators in the polymerase of vinyl halides, such as vinyl chloride or vinyl bromine; vinylidene halides such as vinylene chloride; and other compounds containing polymerizable unsaturated units. The products of this well known poly process have extensive commercial applications. The polymerization of vinyl halides or the copolymerization of vinyl halides with vinylidene halides is usually conducted in an aqueous medium, ie, emulsion, solution or suspension polymerization. In these polymerizations, the monomer or mixture of monomers is dispersed in water in the presence of a sulfactant and subsequently the polymerization is initiated with an organic peroxide. This is a well-known reaction that has been widely reported. All organic peroxides are by nature harmful materials. Its usefulness depends on its ability to decompose into free radicals, illustrated by the following reaction: RO-OR '? RO '+ R O' The speed of this decomposition reaction at any given temperature depends on the structure of R and R '. The decomposition reaction is exothermic. If exothermic decomposition were to occur during production, storage or shipping, when the peroxides are in a concentrated form, excessive pressure and / or fire or explosion may result. Consequently, many organic peroxides must be kept refrigerated. There have been several reports in recent years of the retardation of the decomposition rate of organic peroxides. The Journal of the American Chemical Society, Volume 72, pages 1254 to 1263 (1950), describes the use for example of ethyl acetoacetate, iodine, trinitrobenzene, acetanilide, nitromethane, phenol, hydrogen peroxide and tetralin, to retard the speed of decomposition of diisopropyl peroxydicarbonate.
The patent of the U.S.A. No. 4,515,929 (1985) reports aqueous dispersions of organic peroxides including peroxy dicarbonates, which are stabilized against decomposition by the addition of diphenyl peroxydicarbonate or di (alkyl substituted) phenyl peroxydicarbonates. The patent of the U.S.A. No. 4,552,682 (1985) describes the use of phenolic antioxidants to retard the rate of degradation of aqueous organic peroxide dispersions. The use of phenolic antioxidants is undesirable because they result in discoloration. The patent of the U.S.A. No. 5,155,192 (1992) describes the use of organic hydroperoxides, for example ter-butyl hydroperoxide, to retard the decomposition rate of peroxy dicarbonates. Research Disclosure, April 1995, on page 275, reports the thermal stabilization of dialkyl peroxydicarbonates using unsaturated nitriles or unsaturated acetylenic compounds. COMPENDIUM OF THE INVENTION The present invention relates to the use of certain non-peroxide compounds that are effective in retarding the decomposition rate of organic peroxides such as peroxydicarbonate. Thus, one aspect of the present invention is a composition containing an organic peroxide compound such as a peroxydicarbonate and phosphomolybdic acid which reduces the rate of decomposition of the peroxide compound. Another aspect of the present invention is the method of stabilizing a peroxydicarbonate against decomposition, which comprises adding phosphoric acid in an effective amount to achieve said stabilization. BRIEF DESCRIPTION DETÁt-t-Ar >; A G > The present invention relates to compositions containing an organic peroxide such as a peroxydicarbonate and phosphorandibic acid to retard the decomposition rate of the peroxide compound. Phosphomolybdic acid is a term that refers to any of the various acidic compounds of phosphorus, molybdenum, oxygen and hydrogen. Without intending to be bound by any particular molecular structure or synthesis mode, the phosphomolybdic acid can be illustrated by the formulas H3PM0-0x or H3P04-tmo07dMo02 where (which is equal to (t + d) is typically 10 to 20 but may be higher at 20 or less than 10, and x is typically 34 to 65, but may be greater than 65 or less than 34, and d may be 0. Preferred phosphomolybdic acid for use in the present invention, includes compounds corresponding to the formulas H3P 01204o ( CAS Nos. 12026-57-2 and 51429-74-4, also known as P205-20MoO3xHO), H3PM012020 (CAS Registry No. 99570-13-5) H3P 0lo034 (CAS Registry No. 99559-64-5); and H3PM0lo034 (CAS Registry No. 12519-76-5) Other phospho-olibic acids corresponding to these formulas are also contemplated within the present invention.Olhobic phosphide acid is usually associated with up to about 60 mmoles of water of hydration per mmol of water. phosphomolybdic acid. You can add Phosphomolybdic acid is in solid form but its solubility in economical solvents such as denatured ethanol, makes it practical to use phosphomolybdic acid solutions to add the desired small amounts to the organic peroxide. Other solvents useful in this aspect include other alcohols such as methanol, isopropyl alcohol, n-butanol ethers such as diethyl ethers; glycols such as ethylene glycol; ethers such as ethyl acetate; and ketone such as acetone, methyl ethyl ketone and diethyl ketone. The amount of phosphomolybdic acid for use in the compositions of the present invention is an amount sufficient to retard the rate of decomposition of the peroxide compound. The preferred amount of fssfomolybdic acid is a concentration of .001 to 1.0% and more preferably .02 to .1% by weight of the peroxydicarbonate or other organic peroxide present. When the phosphomolybdic acid is added as a solution, the amount of the solution to be used is adjusted according to the amount of phosphomolybdic acid present in the solution. The exact amount will vary and will depend on the organic peroxide compound and the conditions to which the peroxide composition is to be exposed. Peroxide compounds useful in this invention are of the general structural formula: R 1 - 0 - C (0) - O - C (0) - 0 - R2 wherein R 1 and R 2 each may be an aliphatic, cycloaliphatic or aromatic group with 1 to 22 carbon atoms, preferably 2 to 8 carbon atoms. R1 and R2 can be branched or unbranched, substituted or unsubstituted alkyl, alkenyl, cycloalkyl, or aromatic groups. Examples of groups R1 and R2 include phenyl, methyl, ethyl, n-propyl, isopropyl, n-butyl, sec-butyl, t-butyl, isobutyl, hexyl, octyl, neopentyl, 2-ethylhexyl, capryl, lauryl, myristyl, cetyl , stearyl, allyl, methallyl, crotyl, cyclohexyl, 4-t-butylcyclohexyl, 4-t-amyclohexyl, benzyl, 2-phenylethyl, 2-phenylbutyl, alpha-carbetoxyethyl, beta-methoxyethyl, 2-phenoxyethyl, 2-methoxyphenyl, 3- ethoxyphenyl, 2-ethoxyethyl, 2-ethoxyphenyl, 3-methoxybutyl, 2-carbayloxyethyl, 2-chloroethyl, 2-nitrobutyl, and 2-nitro-2-ethylpropyl. Specific examples of peroxydicarbonates include diethyl peroxydicarbonate, di-n-butyl peroxydicarbonate, di-n-butyl peroxydicarbonate, diisobutyl peroxydicarbonate, disobutilperoperoxydicarbonate and di-4-tert. < "Butylcyclohexyl peroxydicarbonate. Preferably, the peroxycarbonate is di-sec-butylperoxydicarbonate, di-2-ethylhexyl peroxydicarbonate, di-n-propyl peroxydicarbonate or diisopropyl peroxydicarbonate. The peroxide compound can be symmetric or asymmetric, ie R1 and Rz may be the same or different. The peroxide may be a homogeneous mixture containing symmetric peroxides, asymmetric peroxides such as isopropyl-sec-buty1-peroxydicarbonate, or a mixture of symmetric and asymmetric peroxides such as mixtures of diisopropyl peroxydicarbonate, dl-sec-butylperoxydicarbonate and isopropyl-sec-butyl -peroxydicarbonate as described in the US patent No. 4,269,726. The peroxydicarbonate compounds can be synthesized by conventional family techniques to a person of ordinary skill in the art. Peroxydicarbonates are typically prepared by reacting the corresponding alkyl chloroformate with aqueous sodium peroxide at low temperatures, 0 to 20 ° C. The patent of the U.S.A. No. 2,370,588 and the Journal of the American Chemical Society, Volume 72, pages 1254 to 1263 (1950). Other synthetic techniques will be familiar to a person with ordinary skill in the specialty. Preferably, the peroxydicarbonates useful in this invention include those which are liquid at 0 ° C and more preferably a liquid at 5 ° C. Even more preferred are peroxydicarbonates which are liquid up to -20 ° C.
The present invention is especially applicable to aqueous dispersions of peroxydicarbonates which are useful as initiators in the polymerization of free radicals of ethylenically unsaturated materials, particularly in an aqueous medium, for example emulsion or suspension polymerization. A dispersion of the peroxydicarbonate is prepared by dispersing it in water with a convenient dispersing aid, for example a surfactant or emulsifying agent. Surfactants and emulsifying agents useful in the formation of these dispersions are well known in the art and are quite numerous. To prepare dispersions according to the present invention, the phosphomolybdic acid or a solution thereof can be added to an already formed peroxide dispersion, or to the water containing the surfactant, or to the peroxide before the dispersion is formed. Dispersions of the present invention generally contain from 20 to 70% by weight, preferably 30 to 60% by weight of the peroxydicarbonate or other organic peroxide compound and 0.001 to 1.0% (by weight of peroxide) of phosphomolybdic acid. The manner of preparation of the peroxide dispersions is known to a person of ordinary skill in the art. A description of peroxydicarbonate dispersions and their preparation can be found in U.S. Pat. No. 4,515,929; Patent of the U.S.A. Do not. 3,825,509; Patent of the U.S.A. No. 3,988,261 and U.S. Pat. No. 4,092,470. Peroxydicarbonate compositions of the present invention can also be prepared as physical mixtures in the form of liquids, granules, powders or flakes. A physical mixture according to the present invention can be prepared by mixing a liquid peroxide compound or a solution of a peroxide in a convenient solvent, with the desired amount of phosphomolybdic acid or solution thereof in a conventional mixing apparatus. The resulting mixture is then granulated, pulverized or flaked if desired. The phosphomolybdic acid can be added either (1) to the chloroformate-containing reaction mixture before preparation of the peroxide compound or (2) to the unprocessed reaction mixture immediately after preparation of the peroxide compound. Either (1) or (2) will ensure that the two components are mixed as homogeneously as possible in order to receive the greatest possible benefit from the stabilizing effect of the acid of the phosphomolybdic acid. A solution of the present invention can be prepared by combining the desired amounts of phosphomolybdic acid and peroxide in a convenient solvent. Suitable organic solvents include those normally employed for peroxydicarbonates such as esters of phthalic acid, an example of which is dibutyl phthalate and aliphatic and aromatic hydrocarbons and mixtures of these hydrocarbons, examples of which are hexane, odorless mineral spirits, mineral oil, benzene, toluene, xylene, and (iso) paraffins such as isododecane. Other suitable solvents will be familiar to a person with ordinary skill in the specialty. Solutions according to the present invention contain at least 10% and more preferably less than 25% by weight of a peroxydicarbonate compound. The peroxide compositions of the present invention exhibit numerous significant advantages. Primarily among these, improved thermal stability is provided, both in response to exposure to raising the temperature and in response to a given constant temperature. The thermal stability of self-reactive substances, in response to raising temperatures, can be determined by measuring the temperature of self-accelerating decomposition or SADT (SADT = self accelerating decomposition temperature). SADT is one of the recognized tests to determine the transport and safe storage of materials such as organic peroxides. [Transportation recommendations for dangerous goods (Reccomendations on the Transport of Dangerous Goods), ninth edition, United Nations, NY 1995, Section 11.3.5 page 264].
SADT can be correlated directly with the start temperature as measured in a differential thermal analyzer (DTA). The starting temperature is the point at which uncontrolled thermal decomposition begins. The starting temperature can be measured by determining the point at which the rate of temperature increase in a closed cell exceeds a certain pre-determined value. In addition, the start temperature can be measured by determining the point at which the rate of increase in pressure in the closed cell exceeds a certain predetermined value. Thermal stability in response to a given constant temperature can be estimated by accelerated aging tests for example at 15 ° C. Phosphomolybdic acid of the present invention increases at the starting temperature of peroxydicarbonate. Also, the phosphomolybdic acid does not impair the effectiveness of the peroxide as a polymerization initiator. The following examples are intended to illustrate the claimed invention and are in no way designed to limit its scope. Numerous additional embodiments within the scope and spirit of the claimed invention will be apparent to those skilled in the art. EXAMPLE 1 The starting temperature is measured for samples of pure di-2-ethylhexyl peroxydicarbonate, di-2-ethylhexyl peroxydicarbonate diluted in odorless mineral spirits (OMS) and di-sec-butyl peroxydicarbonate diluted in OMS. The starting temperature can also be measured for samples of the aforementioned peroxydicarbonates, in the presence of various amounts of phosphomolybdic acid. The liquid mixtures were prepared by dissolving the required amount of phosphomolybdic acid solution in the peroxydicarbonate. Using a type of Differential Thermal Analyzer (Radex Solo Thermal Analyzer, distributed by Astra Scientific International, Pleasanton, CA.), with an isothermal retention temperature of 30 ° C for 15 minutes and then a temperature increase of 1"/ minute to 130 ° C, the start temperature is measured for a sample of one gram of peroxydicarbonate in a closed cell.The start temperature is measured both by noting the point where the rate of increase (? T) of the sample temperature has reached 0.2 ° C / minute and also the point where the rate of increase in pressure (áP) of the closed sample cell reaches 0.0703 Kg / cm2 (1.0 psi) / minute.eltaT is the difference between the temperature of the oven and the sample temperature. P is the difference between a precalibrated reference pressure and the pressure developed in the sealed sample cell.
The results presented in Table I show that the presence of phosphomolybdic acid increases the temperature at which the self-accelerated decomposition of peroxydicarbonate will begin. This shows that phosphomolybdic acid is an effective stabilizer. Table I. Start temperature for peroxydicarbonates stabilized with phospho-bothic acid (PMA) Peroxide% by weight Temperature of PMA * pure aggregate start (° C) By AT By AP 97.7% Di-2- none 36.3 42.3 ethylhexyl-peroxydicarbonate ( pure) 97.7% Di-2- 0.1 50.2 53.9 ethylhexyl-peroxydicarbonate (pure) 74.8% Di-2- none 41.4 43.6 ethylhexyl peroxydicarbonate in WHO Table I. Starting temperature for peroxydicarbonates stabilized with phosphomolybdic acid (PMA) (Cont.) Peroxide% by weight of Temperature of PMA * pure start added j___C By AT By AP 74. 8% Di-2- 0.62 52.6 53.5 ethylhexyl peroxydicarbonate in WHO 74.8% Dl-2- 0.2 51.5 53.5 ethylhexyl peroxydicarbonate in WHO 74.8% Dl-2- 0.1 53.9 54.2 ethylhexyl peroxydicarbonate in WHO Peroxide% wt. PMA * pure aggregate start t_c_ By AT By AP 74. 8% Di-2- 0.04 52.5 52.0 Ethylhexyl peroxydicarbonate Peroxide% by weight Temperature of PMA * pure start added! ____ By AT By AP in OMS 74.8% Di-2- 0.02 50.4 52.1 ethylhexyl peroxydicarbonate in WHO 74.8% Di -2- 0.01 47.8 47.2 ethylhexyl peroxydicarbonate in WHO 74.8% Di-2- 0.004 44.3 46.5 ethylhexyl peroxydicarbonate in WHO 74.8% Di-2- none 36.6 41.0 ethylhexyl peroxydicarbonate in WHO 74.8% Di-2-1 47.9 51.3 ethylhexyl- Peroxydicarbonate in WHO *: Added as a 20% by weight solution in denatured ethanol. EXAMPLE 2 The effect of the presence of phosphomolybdic acid on storage stability at 15 ° C of pure di-2-ethylhexyl peroxydicarbonate, di-2-ethylhexylperoxydicarbonate diluted in odorless mineral spirits (OMS) and di-sec-butylperoxydicarbonate diluted in OMS, is determined as an accelerated aging test. The purity of the peroxydicarbonate is measured at weekly intervals. The results presented in Table II show that phosphomolybdic acid is an effective stabilizer of peroxydicarbonate. Table II Purity versus time for peroxydicarbonates stabilized with phosphomolybdic acid (PMA) Peroxide% by weight% purity after pure storage PMA * added 1 week 2 weeks 3 weeks 4 weeks 97.7% Di-2- none 37.3 22.4 21.6 18.8 ethylhexyl- peroxydicarbonate (Pure) 97.7% DÍ-2- 0.1 94.7 84.0 76.7 69.4 ethylhexyl-Table II Purity against time for peroxydicarbonates stabilized with phosphomolybdic acid (PMA) Peroxide% by weight% purity after pure storage PMA * added 1 week 2 weeks 3 weeks 4 weeks peroxydicarbonate (pure) 74.8% Di-2- none 28.6 17.9 15.4 14.9 ethylhexyl peroxydicarbonate in WHO 74.8% Di-2- 0.1 70.1 64.0 57.8 53.2 ethylhexyl peroxydicarbonate in WHO Peroxide% in weight% purity after of pure storage PMA * added 1 week 2 weeks 3 weeks 4 weeks 76. 2% Di-2- none 19.9 17.7 18.2 19.4 secbutyl peroxydicarbonate in WHO Peroxide% by weight% pure after storage PMA * added 1 week 2 weeks 3 weeks 4 weeks 76.2% Di- 0.1 60.1 46.6 39.5 37.5 sec- peroxydicarbonate in WHO *: added as a 20% by weight solution in denatured ethanol.

Claims (16)

  1. CLAIMS 1. A composition characterized in that it comprises: (a) an organic peroxide component selected from the group consisting of peroxydicarbonate compounds and their mixtures; and (b) a sufficient amount of phosphomolybdic acid to retard the decomposition rate of the organic peroxide component.
  2. 2. A composition according to claim 1, characterized in that the organic peroxide component comprises at least one compound of the formula (i) R1-O-C (O) - 0-C (O) -O-R2 in where R1 and R2 independently are aliphatic, cycloaliphatic or aromatic groups containing 1 to 22 carbon atoms.
  3. 3. A composition according to claim 2, characterized in that R1 and R2 are independently selected from the group consisting of: phenyl, methyl, ethyl, n-propyl, isopropyl, n-butyl, sec-butyl, t-butyl, isobutyl, hexyl, octyl, neopentyl, 2-ethylhexyl, capryl, lauryl, iristyl, cetyl, stearyl, allyl, methallyl, crotyl, cyclohexyl, 4-t-butylcyclohexyl, 4-ta icliohexyl, benzyl, 2-phenylethyl, 2-phenylbutyl , alpha-carbetoxyethyl, beta-methoxyethyl, 2-phenoxyethyl, 2-methoxyphenyl, 3-methoxyphenyl, 2-ethoxyethyl, 2-ethoxyphenyl, 3-methoxybutyl, 2-carbamyloxyethyl, 2-chloroethyl, 2-nitrobutyl, and 2-nitro-2 -methylpropyl.
  4. 4. Composition according to claim 1, characterized in that the organic peroxide component is selected from the group consisting of: diethyl peroxydicarbonate, isopropyl-sec-butyl-but idicarbonate, di-n-butyl-peroxydicarbonate, diisobutyl peroxydicarbonate, di -4-tert-butylcyclohexyl peroxydicarbonate, di-2-ethylhexyl peroxydicarbonate, di-n-propyl peroxydicarbonate, diisopropyl peroxydicarbonate, and mixtures thereof.
  5. 5. Composition according to claim 1, characterized in that the phosphomolybdic acid comprises 0.001 to 1.0% by weight of the organic peroxide component.
  6. 6. Compositions according to claim 5, characterized in that the phosphomolybdic acid comprises 0.02 to 0.1% by weight of the organic peroxide component.
  7. 7. Compositions according to claim 2, characterized in that the phosphomolybdic acid comprises 0.001 to 1.0% by weight of the organic peroxide component.
  8. 8. Compositions according to claim 7, characterized in that the phosphomolybdic acid comprises 0.02 to 0.1% by weight of the organic peroxide component.
  9. 9. Method for retarding the decomposition rate of an organic peroxide product, selected from the group consisting of peroxydicarbonate compounds and their mixtures, characterized in that it comprises adding to the organic peroxide compound phosphomolybdic acid in an amount effective to retard the rate of decomposition.
  10. 10. Method according to claim 9, characterized in that the peroxydicarbonate compounds correspond to the formula (I): Rx-O-C (O) -O-C (O) -O-R2 wherein R1 and R2 independently they are cycloaliphatic or aromatic aliphatic groups containing 1 to 22 carbon atoms.
  11. 11. Method according to claim 10, characterized in that R1 and R2 are independently selected from the group consisting of: phenyl, methyl, ethyl, n-propyl, isopropyl, n-butyl, sec-butyl, t-butyl, isobutyl hexyl, octyl, neopentyl, 2-ethylhexyl, capryl, lauryl, iristyl, cetyl, stearyl, allyl, ratetalyl, crotyl, cyclohexyl, 4-t-butylcyclohexyl, 4-t-amylcyclohexyl, benzyl, 2-phenylethyl, 2-phenylbutyl , alpha-carbetoxyethyl, beta-methoxyethyl, 2-phenoxyethyl, 2-methoxyphenyl, 3-methoxyphenyl, 2-ethoxyethyl, 2-ethoxyphenyl, 3-ethoxybutyl, 2-carbamyloxyethyl, 2-chloroethyl, 2-nitrobutyl, and 2-nitro 2-methylpropyl.
  12. 12. - Method according to claim 9, characterized in that the organic peroxide component is selected from the group consisting of: diethyl peroxydicarbonate, isopropyl-sec-butyl-but-idicarbonate, di-n-buty 1-peroxydicarbonate, dissectyl peroxydicarbonate, 4-tert-butylcyclohexyl peroxydicarbonate, di-2-ethylhexyl peroxydicarbonate, di-n-propyl peroxydicarbonate, diisopropyl peroxydicarbonate, and mixtures thereof.
  13. 13. Method according to claim 9, characterized in that the amount of the phosphomolybdic acid is 0.001 to 1.0% by weight of the organic peroxide product.
  14. 14. Method according to claim 13, characterized in that the amount of the phosphomolybdic acid is 0.02 to 0.1% by weight of the organic peroxide product.
  15. 15. Method according to claim 10, characterized in that the amount of the phosphomolybdic acid is 0.001 to 1.0% by weight of the organic peroxide product.
  16. 16. Method according to claim 15, characterized in that the amount of the phosphomolybdic acid is 0.02 to 0.1% by weight of the organic peroxide product.
MXPA/A/1997/003994A 1996-05-31 1997-05-30 Stabilization of organic peroxide with fosfomolibd acid MXPA97003994A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US08/656,095 US5719304A (en) 1996-05-31 1996-05-31 Organic peroxide stabilization with phosphomolybdic acid
US08656095 1996-05-31

Publications (2)

Publication Number Publication Date
MX9703994A MX9703994A (en) 1998-06-30
MXPA97003994A true MXPA97003994A (en) 1998-10-30

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